Cloud Condensation Nuclei Number Concentration Research Articles

Consistency and applicability of parameterization schemes for the size-resolved aerosol activation ratio based on field measurements in the North China Plain

Parameterization of the size-resolved particle activation ratio (AR) is useful for the prediction and analysis of the cloud condensation nuclei (CCN) number concentration (NCCN). Critical issues for the application of AR parameterizations in models are (1) the consistency of the different parameterization schemes in terms of fitting AR curves and (2) the applicability of the estimate of NCCN under different aerosol conditions. These issues are discussed in this study based on summertime measurements of the size-resolved AR in the North China Plain. By comparing parameterized AR curves, variations in the fitting parameters and application to NCCN calculations, the consistency of the three existing parameterization schemes is confirmed. Based on an analysis using representative AR fitting parameters, the method commonly used to calculate NCCN with a fixed AR was found to be accurate, except during periods affected by strong black carbon (BC) emissions or new particle formation (NPF) events. The NCCN value was overestimated by approximately 10% when BC aerosol emissions were abundant and deviated from the 1:1 line by 15% during NPF events. The bias of the calculated NCCN due to these significant emission or aerosol production events cannot be eliminated by using the appropriate representative fitting parameters. Under these circumstances, accurate prediction of NCCN requires real-time aerosol hygroscopicity data based on CCN measurements. This research furthers our understanding of the relationship between aerosol cloud activation and aerosol spectra.

Airborne observations of cloud condensation nuclei spectra and aerosols over East Inner Mongolia

A set of vertical profiles of aerosol number concentrations, size distributions and cloud condensation nuclei (CCN) spectra was observed using a passive cloud and aerosol spectrometer (PCASP) and cloud condensation nuclei counter, over the Tongliao area, East Inner Mongolia, China. The results showed that the average aerosol number concentration in this region was much lower than that in heavily polluted areas. Monthly average aerosol number concentrations within the boundary layer reached a maximum in May and a minimum in September, and the variations in CCN number concentrations at different supersaturations showed the same trend. The parameters c and k of the empirical function N = cS k were 539 and 1.477 under clean conditions, and their counterparts under polluted conditions were 1615 and 1.42. Measurements from the airborne probe mounted on a Yun-12 (Y12) aircraft, together with Hybrid Single-Particle Lagrangian Integrated Trajectory model backward trajectories indicated that the air mass from the south of Tongliao contained a high concentration of aerosol particles (1000–2500 cm−3) in the middle and lower parts of the troposphere. Moreover, detailed intercomparison of data obtained on two days in 2010 indicated that the activation efficiency in terms of the ratio of N CCN to N a (aerosols measured from PCASP) was 0.74 (0.4 supersaturations) when the air mass mainly came from south of Tongliao, and this value increased to 0.83 on the relatively cleaner day. Thus, long-range transport of anthropogenic pollutants from heavily polluted mega cities, such as Beijing and Tianjin, may result in slightly decreasing activation efficiencies.

CCN characteristics over a tropical coastal station during south-west monsoon: observations and closure studies

Number concentration measurements of cloud condensation nuclei (CCN) at five supersaturation values between 0.2 and 1.0% were made from a coastal site (Thiruvananthapuram) of peninsular India using a single column CCN counter during the summer monsoon period (June–September) of 2013 and 2014. The CCN concentration over this site showed diurnal variations of high values during nighttime and low values during daytime in association with the change in mesoscale circulation patterns. The inter-annual variations of CCN (CCN0.4% = 2,232 ± 672 cm−3 during August 2013 and CCN0.4% = 941 ± 325 cm−3 during August 2014) are mostly associated with the varying intensity of monsoon rainfall. The variation of CCN number concentration with supersaturation is found to be steeper during nighttime (indicating a less CCN active aerosol system) than during daytime (CCN active system). The CCN activation ratio estimated using simultaneous measurements of CCN and aerosol number (CN) concentration clearly depict the role of land-sea breeze circulations with higher values during daytime than the nighttime. The CCN number concentration predicted for different supersaturations, from measured aerosol number size distribution using Kohler theory, indicate the importance of the change in aerosol composition associated with different airmasses in a coastal environment.

Surface tension prevails over solute effect in organic-influenced cloud droplet activation.

The spontaneous growth of cloud condensation nuclei (CCN) into cloud droplets under supersaturated water vapour conditions is described by classic Köhler theory. This spontaneous activation of CCN depends on the interplay between the Raoult effect, whereby activation potential increases with decreasing water activity or increasing solute concentration, and the Kelvin effect, whereby activation potential decreases with decreasing droplet size or increases with decreasing surface tension, which is sensitive to surfactants. Surface tension lowering caused by organic surfactants, which diminishes the Kelvin effect, is expected to be negated by a concomitant reduction in the Raoult effect, driven by the displacement of surfactant molecules from the droplet bulk to the droplet-vapour interface. Here we present observational and theoretical evidence illustrating that, in ambient air, surface tension lowering can prevail over the reduction in the Raoult effect, leading to substantial increases in cloud droplet concentrations. We suggest that consideration of liquid-liquid phase separation, leading to complete or partial engulfing of a hygroscopic particle core by a hydrophobic organic-rich phase, can explain the lack of concomitant reduction of the Raoult effect, while maintaining substantial lowering of surface tension, even for partial surface coverage. Apart from the importance of particle size and composition in droplet activation, we show by observation and modelling that incorporation of phase-separation effects into activation thermodynamics can lead to a CCN number concentration that is up to ten times what is predicted by climate models, changing the properties of clouds. An adequate representation of the CCN activation process is essential to the prediction of clouds in climate models, and given the effect of clouds on the Earth's energy balance, improved prediction of aerosol-cloud-climate interactions is likely to result in improved assessments of future climate change.

Aerosol physicochemical effects on CCN activation simulated with the chemistry-climate model EMAC

This study uses the EMAC atmospheric chemistry-climate model to simulate cloud properties with a prognostic cloud droplet nucleation scheme. We present modeled global distributions of cloud condensation nuclei (CCN) number concentrations and CCN activation rates, together with the effective hygroscopicity parameter κ, to describe the aerosol chemical composition effect on CCN activation. Large particles can easily activate into cloud droplets, even at low κ values due to the dominant size effect in cloud droplet formation. Small particles are less efficiently activated as CCN, and are more sensitive to aerosol composition and supersaturation. Since the dominant fraction of small particles generally originates from anthropogenic precursor emissions over land, this study focuses on the influence of the continental atmosphere, using a prognostic cloud droplet nucleation scheme that considers aerosol-cloud interactions during cloud formation, together with a double-moment cloud microphysics scheme. The agreement of simulated clouds and climate with observations generally improves over the Northern Hemisphere continents, particularly high air pollution regions such as Eastern US, Europe, East Asia by accounting for aerosol-cloud interactions that include impacts of chemical composition on CCN activation.

Hygroscopicity and cloud condensation nucleus activity of forest aerosol particles during summer in Wakayama, Japan

AbstractSize‐resolved distributions of the hygroscopic growth factor (g) and the ratios of cloud condensation nuclei (CCN) to condensation nuclei were observed at a forest site during summer in Japan. The g distributions at 85% relative humidity were unimodal. During 0900–2100 Japan Standard Time (JST) on new particle formation (NPF) event days, less hygroscopic particles (g ~ 1.1) were dominant in the Aitken‐mode range and the CCN activation diameters of the aerosols were large. These results are explained by the substantial contribution from newly formed biogenic secondary organic aerosol (BSOA). Hygroscopicity parameter κ for newly formed Aitken particles, calculated from g and CCN activation diameters, were 0.12 and 0.16, respectively, which were estimated to be the κ of organics. The κ values of particles were higher during 2100–0900 JST on NPF event days, in which the aerosols were characterized by the dominance of large and more hygroscopic particles. The number fractions of CCN that were predicted from time‐ and size‐resolved g at 0.23% and 0.41% supersaturations better matched the measured values compared to the cases with the time‐averaged g and/or g for the bulk composition, which suggests that the differences in particle hygroscopicity with time and size are important to CCN activation. A cloud parcel model indicates that the contributions from less hygroscopic particles to the number concentrations of CCN and cloud droplets were potentially large during NPF event days, which suggests a marked contribution from locally formed BSOA particles alongside particles from background air.

Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

CCN production by new particle formation in the free troposphere

Abstract. Global models predict that new particle formation (NPF) is, in some environments, responsible for a substantial fraction of the total atmospheric particle number concentration and subsequently contributes significantly to cloud condensation nuclei (CCN) concentrations. NPF events were frequently observed at the highest atmospheric observatory in the world, on Chacaltaya (5240 m a.s.l.), Bolivia. The present study focuses on the impact of NPF on CCN population. Neutral cluster and Air Ion Spectrometer and mobility particle size spectrometer measurements were simultaneously used to follow the growth of particles from cluster sizes down to ∼ 2 nm up to CCN threshold sizes set to 50, 80 and 100 nm. Using measurements performed between 1 January and 31 December 2012, we found that 61 % of the 94 analysed events showed a clear particle growth and significant enhancement of the CCN-relevant particle number concentration. We evaluated the contribution of NPF, relative to the transport and growth of pre-existing particles, to CCN size. The averaged production of 50 nm particles during those events was 5072, and 1481 cm−3 for 100 nm particles, with a larger contribution of NPF compared to transport, especially during the wet season. The data set was further segregated into boundary layer (BL) and free troposphere (FT) conditions at the site. The NPF frequency of occurrence was higher in the BL (48 %) compared to the FT (39 %). Particle condensational growth was more frequently observed for events initiated in the FT, but on average faster for those initiated in the BL, when the amount of condensable species was most probably larger. As a result, the potential to form new CCN was higher for events initiated in the BL (67 % against 53 % in the FT). In contrast, higher CCN number concentration increases were found when the NPF process initially occurred in the FT, under less polluted conditions. This work highlights the competition between particle growth and the removal of freshly nucleated particles by coagulation processes. The results support model predictions which suggest that NPF is an effective source of CCN in some environments, and thus may influence regional climate through cloud-related radiative processes.

Size-resolved aerosol and cloud condensation nuclei (CCN) properties in the remote marine South China Sea – Part 1: Observations and source classification

Abstract. Ship-based measurements of aerosol and cloud condensation nuclei (CCN) properties are presented for 2 weeks of observations in remote marine regions of the South China Sea/East Sea during the southwestern monsoon (SWM) season. Smoke from extensive biomass burning throughout the Maritime Continent advected into this region during the SWM, where it was mixed with anthropogenic continental pollution and emissions from heavy shipping activities. Eight aerosol types were identified using a k-means cluster analysis with data from a size-resolved CCN characterization system. Interpretation of the clusters was supplemented by additional onboard aerosol and meteorological measurements, satellite, and model products for the region. A typical bimodal marine boundary layer background aerosol population was identified and observed mixing with accumulation mode aerosol from other sources, primarily smoke from fires in Borneo and Sumatra. Hygroscopicity was assessed using the κ parameter and was found to average 0.40 for samples dominated by aged accumulation mode smoke; 0.65 for accumulation mode marine aerosol; 0.60 in an anthropogenic aerosol plume; and 0.22 during a short period that was characterized by elevated levels of volatile organic compounds not associated with biomass burning impacts. As a special subset of the background marine aerosol, clean air masses substantially scrubbed of particles were observed following heavy precipitation or the passage of squall lines, with changes in observed aerosol properties occurring on the order of minutes. Average CN number concentrations, size distributions, and κ values are reported for each population type, along with CCN number concentrations for particles that activated at supersaturations between 0.14 and 0.85 %.

Influences of aerosol physiochemical properties and new particle formation on CCN activity from observation at a suburban site of China

With the aim of understanding the impact of aerosol particle size and chemical composition on CCN activity, the size-resolved cloud condensation nuclei (CCN) number concentration (NCCN), particle number size distribution (PSD) (10–600nm), and bulk chemical composition of particles with a diameter <1.0μm (PM1) were measured simultaneously at Xinzhou, a suburban site in northern China, from 22 July to 26 August 2014. The NCCN was measured at five different supersaturations (SS) ranging from 0.075%–0.76%. Diurnal variations in the aerosol number concentration (NCN), NCCN, the bulk aerosol activation ratio (AR), the hygroscopicity parameter (κchem), and the ratio of 44 mass to charge ration (m/z 44) to total organic signal in the component spectrum (f44), and the PSD were examined integrally to study the influence of particle size and chemical composition on CCN activation. We found that particle size was more related to the CCN activation ratios in the morning, whereas in the afternoon (~1400 LST), κchem and f44 were more closely associated with the bulk AR. Assuming the internal mixing of aerosol particles, NCCN was estimated using the bulk chemical composition and real-time PSD. We found that the predicted CCN number concentrations were underestimated by 20–30% at SS <0.2% probably due to the measurement uncertainties. Estimates were more accurate at higher SS levels, suggesting that the hygroscopicity parameter based on bulk chemical composition information can provide a good estimate of CCN number concentrations. We studied the impacts of new particle formation (NPF) events on size-resolved CCN activity at the “growth” stage and “leveling-off” stage during a typical NPF event by comparing with the case during non-NPF event. It has been found that CCN activation was restrained at the “growth” stage during which larger particle diameters were needed to reach an activation diameter(Da), and the bulk AR decreased as well. However, during the “leveling-off” stage, a lower Da was observed and CCN activation was greatly enhanced.

Thermodynamic properties of nanoparticles during new particle formation events in the atmosphere of North China Plain

To better understand the sources, formation, and the transport of air pollutants over North China Plain (NCP), a four-week intensive campaign during summertime in 2014 was conducted in a central NCP rural site. In this study, particle hygroscopicity and volatility measurements were focused to characterize the thermodynamic properties of nanoparticles and gain insight into chemical composition of nanoparticles during the new particle formation (NPF) events. The water-soluble fractions of 30 and 50nm newly formed particles were respectively 0.64±0.06 and 0.61±0.06, indicating that the water-soluble chemical compounds, most likely ammonium sulfate, dominated the condensational growth of newly formed particles over the NCP. Due to containing higher water-soluble fraction, nanoparticles can be activated as cloud condensation nuclei (CCN) at lower supersaturation in the atmosphere of NCP in contrast to cleaner environments, such as Melpitz (Central European background) and Hyytiälä (boreal forest) during the NPF events. Our observations showed that the NPF and subsequent growth significantly resulted in an enhancement in CCN number concentration. The ranges of enhancement factors of CCN number concentration for supersaturation (SS)=0.2, 0.4, 0.8% were respectively 1.9–7.0, 2.7–8.4, and 3.6–10.1. After being heated to 300°C, the shrink factors for 30 and 50nm particles were respectively 0.35 and 0.38. This indicated that non-volatile compounds could be produced during the growth process of newly formed particles.

Long-term observations of cloud condensation nuclei in the Amazon rain forest – Part 1: Aerosol size distribution, hygroscopicity, and new model parametrizations for CCN prediction

Abstract. Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in the central Amazon Basin over a 1-year period and full seasonal cycle (March 2014–February 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site.The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.For modeling purposes, we compare different approaches of predicting CCN number concentration and present a novel parametrization, which allows accurate CCN predictions based on a small set of input data.

Parameterizing cloud condensation nuclei concentrations during HOPE

Abstract. An aerosol model was used to simulate the generation and transport of aerosols over Germany during the HD(CP)2 Observational Prototype Experiment (HOPE) field campaign of 2013. The aerosol number concentrations and size distributions were evaluated against observations, which shows satisfactory agreement in the magnitude and temporal variability of the main aerosol contributors to cloud condensation nuclei (CCN) concentrations. From the modelled aerosol number concentrations, number concentrations of CCN were calculated as a function of vertical velocity using a comprehensive aerosol activation scheme which takes into account the influence of aerosol chemical and physical properties on CCN formation. There is a large amount of spatial variability in aerosol concentrations; however the resulting CCN concentrations vary significantly less over the domain. Temporal variability is large in both aerosols and CCN. A parameterization of the CCN number concentrations is developed for use in models. The technique involves defining a number of best fit functions to capture the dependence of CCN on vertical velocity at different pressure levels. In this way, aerosol chemical and physical properties as well as thermodynamic conditions are taken into account in the new CCN parameterization. A comparison between the parameterization and the CCN estimates from the model data shows excellent agreement. This parameterization may be used in other regions and time periods with a similar aerosol load; furthermore, the technique demonstrated here may be employed in regions dominated by different aerosol species.

Key features of new particle formation events at background sites in China and their influence on cloud condensation nuclei

Long-term continuous measurements of particle number size distributions with mobility diameter sizes ranging from 3 to 800 nm were performed to study new particle formation (NPF) events at Shangdianzi (SDZ), Mt. Tai (TS), and Lin’an (LAN) stations representing the background atmospheric conditions in the North China Plain (NCP), Central East China (CEC), and Yangtze River Delta (YRD) regions, respectively. The mean formation rate of 3-nm particles was 6.3, 3.7, and 5.8 cm–3∙s–1, and the mean particle growth rate was 3.6, 6.0, and 6.2 nm∙h–1 at SDZ, TS, and LAN, respectively. The NPF event characteristics at the three sites indicate that there may be a stronger source of low volatile vapors and higher condensational sink of pre-existing particles in the YRD region. The formation rate of NPF events at these sites, as well as the condensation sink, is approximately 10 times higher than some results reported at rural/urban sites in western countries. However, the growth rates appear to be 1–2 times higher. Approximately 12%–17% of all NPF events with nucleated particles grow to a climaterelevant size (>50 nm). These kinds of NPF events were normally observed with higher growth rate than the other NPF cases. Generally, the cloud condensation nuclei (CCN) number concentration can be enhanced by approximately a factor of 2–6 on these event days. The mean value of the enhancement factor is lowest at LAN (2–3) and highest at SDZ (~4). NPF events have also been found to have greater impact on CCN production in China at the regional scale than in the other background sites worldwide.

Variation of CCN activity during new particle formation events in the North China Plain

Abstract. The aim of this investigation was to obtain a better understanding of the variability of the cloud condensation nuclei (CCN) activity during new particle formation (NPF) events in an anthropogenically polluted atmosphere of the North China Plain (NCP). We investigated the size-resolved activation ratio as well as particle number size distribution, hygroscopicity, and volatility during a 4-week intensive field experiment in summertime at a regional atmospheric observatory in Xianghe. Interestingly, based on a case study, two types of NPF events were found, in which the newly formed particles exhibited either a higher or a lower hygroscopicity. Therefore, the CCN activity of newly formed particles in different NPF events was largely different, indicating that a simple parameterization of particle CCN activity during NPF events over the NCP might lead to poor estimates of CCN number concentration (NCCN). For a more accurate estimation of the potential NCCN during NPF events, the variation of CCN activity has to be taken into account. Considering that a fixed activation ratio curve or critical diameter are usually used to calculate NCCN, the influence of the variation of particle CCN activity on the calculation of NCCN during NPF events was evaluated based on the two parameterizations. It was found that NCCN might be underestimated by up to 30 % if a single activation ratio curve (representative of the region and season) were to be used in the calculation; and might be underestimated by up to 50 % if a fixed critical diameter (representative of the region and season) were used. Therefore, we suggest not using a fixed critical diameter in the prediction of NCCN in NPF. If real-time CCN activity data are not available, using a proper fixed activation ratio curve can be an alternative but compromised choice.

Impacts of organic aerosols and its oxidation level on CCN activity from measurement at a suburban site in China

Abstract. This study is concerned with the impacts of organic aerosols on cloud condensation nuclei (CCN) activity based on field measurements made at a suburban site in Northern China. The sensitivity of the estimated CCN number concentration (NCCN) to both volume fraction of organic material (xorg) and aerosol oxidation level (using f44, the fraction of m∕z 44 in aerosol organic material) are examined. A strong dependence of CCN number concentration (NCCN) on the xorg and f44 was noted. The sensitivity of NCCN to volume fraction of organics increased with increasing xorg. The impacts of the aerosol particles oxidization or aging level on estimating NCCN were also very significant. When the particles were mostly composed of organics (xorg &gt; 60 %), the NCCN at the supersaturation of 0.075 and 0.13 % was underestimated by 46 and 44 %, respectively, if aerosol particles were freshly emitted with primary organics (f44 &lt; 11 %); the underestimation decreased to 32 and 23 % at the corresponding supersaturations, however, if the particles were with more hygroscopic secondary organics (f44 &gt; 15 %). The NCCN at the supersaturation of 0.76 % was underestimated by 11 and 4 %, respectively, at f44 &lt; 11 and f44 &gt; 15 %. However, for the particles composed of low organics (e.g., xorg &lt; 40 %), the effect caused by the f44 was quite insignificant both at high and low supersaturations. This is because the overall hygroscopicity of the particles is dominated by inorganics such as sulfate and nitrate, which are more hygroscopic than organic compounds. Our results indicated that it would decrease the uncertainties in estimating NCCN and lead to a more accurate estimation of NCCN to increase the proportion of secondary organics, especially when the composition of the aerosols is dominated by organics. The applicability of the CCN activation spectrum obtained at Xinzhou to the Xianghe site, about 400 km to the northeast of Xinzhou, was investigated, with the aim of further examining the sensitivity of NCCN to aerosol type. Overall, the mean CCN efficiency spectrum derived from Xinzhou performs well at Xianghe when the supersaturation levels are &gt; 0.2 % (overestimation of 2–4 %). However, NCCN was overestimated by ∼ 20 % at supersaturation levels of &lt; 0.1 %. This suggests that the overestimation is mainly due to the smaller proportion of aged and oxidized organic aerosols present at Xianghe compared to Xinzhou.

Hygroscopicity and CCN activity of atmospheric aerosol particles and their relation to organics: Characteristics of urban aerosols in Nagoya, Japan

AbstractThe size‐resolved distributions of hygroscopic growth factor g and the ratios of cloud condensation nuclei (CCN) to condensation nuclei of atmospheric aerosols were investigated in Nagoya, Japan. The average of the distributions of g at 85% relative humidity was bimodal. The size‐resolved mean κ derived from g showed an increasing trend with diameter: 0.17–0.33 at 24–359 nm. The κ values calculated from CCN activation curves were 37% higher than those derived from g. Only 9% of the 37% difference is explained by the difference in the κ of inorganics under subsaturated and supersaturated conditions, suggesting a contribution of organics to the remaining 28% difference. The size‐averaged κ of organics (κorg) was calculated as 0.14 and 0.19 by two different methods. The number fractions of CCN predicted from the hygroscopicity data over the range of 24–359 nm are loosely consistent with those observed if the size‐ and time‐averaged g is applied to all particles (differences: −30% to +10%). This consistency improves if size‐ and time‐resolved g and g distribution are used (differences: −19% to −3%). Whereas the number fractions of CCN predicted from the composition data are greatly underestimated if organics are assumed to be insoluble (differences: −64% to −45%), they are more consistent if κorg of 0.14 or 0.19 is applied (differences: −10% to +14%). The results demonstrate the importance of the dependence of the g of particles on time and particle size and the hygroscopicity of organics for CCN number concentrations in the urban atmosphere.

Properties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic

Abstract. Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.

Particle Growth and Variation of Cloud Condensation Nucleus Activity on Polluted Days with New Particle Formation: A Case Study for Regional Air Pollution in the PRD Region, China

ABSTRACTNew particle formation (NPF) events on polluted days at a regional supersite in the Pearl River Delta (PRD) region and its impact on the abundance and properties of cloud condensation nuclei (CCN) were investigated. Nucleation and subsequent significant growth of nanoparticles on a regional scale was observed and representative events on 2 and 6 October 2013 were chosen in this study. The measurements showed that the primary components of the particles were sulfate, ammonium, and organics as they were added continuously to secondary aerosol mass and that particles show inversion from growth to shrink if the particles comprise primarily of organics due to evaporation of semi-volatile species under favorable meteorological conditions. The effective hygroscopicity parameter κ of fine particles on 2 October composed of sulfate, nitrate and ammonium (κ = 0.26–0.42) was larger than that of fine particles on 6 October containing more organics (κ = 0.19–0.36). Particles in the nucleation mode were observed to grow rapidly to the CCN sizes and dominate the CCN number concentrations at a water vapor supersaturation (S) over 0.46%. At an S range of 0.26–0.86%, the CCN number concentrations reached maximum values of (1.3–2.6) × 104 cm–3 after the NPF event on 2 October. The sulfate component in the particles was found to increase significantly, about 50% higher than that before NPF. Results from events on 6 October showed a significant increase of the organic component and the CCN number concentrations after the NPF event were comparable or slightly lower than those before the event. Nevertheless, the average CCN number concentrations scaled with EC mass concentration with S over 0.46% in the daytime of 2 and 6 October were significantly higher than those on a non-NPF event day.

Some insights into the condensing vapors driving new particle growth to CCN sizes on the basis of hygroscopicity measurements

Abstract. New particle formation (NPF) and growth is an important source of cloud condensation nuclei (CCN). In this study, we investigated the chemical species driving new particle growth to the CCN sizes on the basis of particle hygroscopicity measurements carried out at the research station Melpitz, Germany. Three consecutive NPF events occurred during summertime were chosen as examples to perform the study. Hygroscopicity measurements showed that the (NH4)2SO4-equivalent water-soluble fraction accounts for 20 and 16 % of 50 and 75 nm particles, respectively, during the NPF events. Numerical analysis showed that the ratios of H2SO4 condensational growth to the observed particle growth were 20 and 13 % for 50 and 75 nm newly formed particles, respectively. Aerosol mass spectrometer measurements showed that an enhanced mass fraction of sulfate and ammonium in the newly formed particles was observed when new particles grew to the sizes larger than 30 nm shortly after the particle formation period. At a later time, the secondary organic species played a key role in the particle growth. Both hygroscopicity and aerosol mass spectrometer (AMS) measurements and numerical analysis confirmed that organic compounds were major contributors driving particle growth to CCN sizes. The critical diameters at different supersaturations estimated using AMS data and κ-Köhler theory increased significantly during the later course of NPF events. This indicated that the enhanced organic mass fraction caused a reduction in CCN efficiency of newly formed particles. Our results implied that the CCN production associated with atmospheric nucleation may be overestimated if assuming that newly formed particles can serve as CCN once they grow to a fixed particle size, an assumption made in some previous studies, especially for organic-rich environments. In our study, the enhancement in CCN number concentration associated with individual NPF events were 63, 66, and 69 % for 0.1, 0.4, and 0.6 % supersaturation, respectively.